Printed organic thin-film transistors (OTFTs) have received great interest as potentially low-cost alternative to silicon technology for application in large-area, flexible, and ultra-lowcost electronics. The development of printable materials including semiconductor, conductor, and gate dielectric are essential to enable this technology transition. The Xerox efforts in design and development of thiophene-based polymeric semiconductors, metal nanoparticles as printable conductors, and a dual-layer robust gate dielectric materials for all solution-processed highperformance OTFTs will be reviewed in this paper.